SearcharxivSearch

arXiv subjects

Frank Vollmer

Publications and source records attributed to Frank Vollmer.

15 recordsLinked to original sources

Single-nanoparticle detection using quasi-bound states in the continuum supported by silicon metasurfaces

The detection of single particles or molecules represents a critical milestone in the development of biosensing technologies. Recently developed optical sensors based on quasi-bound states in the continuum (qBICs) have primarily focused on detecting global refractive index changes, aiming to simultaneously enhance both refractive index sensitivity and quality ($Q$) factors. However, sensors capable of resolving local refractive index perturbations, such as the binding of a nanometer-sized molecule on a surface, remain elusive and have not yet been demonstrated in BIC geometries due to the limited $Q$ factors and relatively large mode volumes. Here, we demonstrate low-contrast BIC metasurfaces that can perform sensing with a virus-sized single-nanoparticle resolution. The qBIC resonance operating at the critical coupling condition exhibits an experimental $Q$ factor of 4.5 x 10$^4$ in heavy water. The strong interaction between the localized electric field and polystyrene nanoparticles with a diameter of 100 nm enable the experimental observation of step-like resonance wavelength shifts, serving as signatures of individual particle binding events. Furthermore, binding-induced modifications to the qBIC resonance alter the optical confinement and asymmetry factor, inducing changes not only in the resonance wavelength but also in the linewidth and amplitude with single-particle sensitivity. Combined with position-insensitive response and free-space accessible features, low-contrast BIC metasurfaces provide a user-friendly platform for next-generation single-molecule sensing integrated with microfluidic systems.

physics.optics

Probing the single neurotransmitters with the WGM microcavity-hybridized plasmonic nanospiked antennas

Discerning the neurotransmitter dysregulation is a hallmark of neurological disorders and diseases, including Alzheimer's, Parkinson's, and multiple sclerosis. The concentration of neurotransmitters in the synaptic cleft is particularly low, ranging from nM to fM, which makes it challenging to accurately monitor changes over the course of a clinical trial using existing sensing techniques. By means of an advanced whispering gallery mode (WGM) sensor hybridized with plasmonic nanospiked antennas, we detect and discriminate between different neurotransmitters at the single-molecule level. Our results show that the sensor can detect neurotransmitters with exceptional sensitivity down to 10 aM and discriminate between structurally similar neurotransmitters, such as GABA and glutamate, over a large number of detection events. Furthermore, we find that the average WGM resonance shift, induced by a neurotransmitter binding to the sensor, strongly correlates with molecular polarizability values obtained from electronic structure calculations. These findings establish the optoplasmonic WGM sensors as potential biosensor platform in different avenues of neuroscience by detecting and discriminating neurotransmitters as well as investigating their dynamics at ultra low-level concentrations, plausibly contributing to deeper understanding of brain function and neurological disorders.

physics.bio-ph

Monitoring Single DNA Docking Site Activity With Sequential Modes of an Optoplasmonic Whispering-Gallery Mode Biosensor

In recent years, there has been rapid advancement in single-molecule techniques, driven by their unparalleled precision in studying molecules whose sizes are beyond the diffraction limit. Among these techniques, optoplasmonic whispering gallery mode sensing has demonstrated great potential in label-free single-molecule characterization. It combines the principles of localized surface plasmon resonance (LSPR) and whispering gallery mode (WGM) sensing, offering exceptional sensing capabilities, even at the level of single ions. However, current optoplasmonic WGM sensing operates in a multiplexed channel, making it challenging to focus on individual binding sites of analyte molecules. In this article, we characterize different binding sites of DNA analyte molecules hybridizing to docking strands on the optoplasmonic WGM sensor, using the ratio of the resonance shift between sequential polar WGM modes. We identify specific docking sites that undergo transient interactions and eventually hybridize with the complementary analyte strands permanently.

physics.bio-ph

Enhanced Whispering Gallery Mode Phase Shift using Indistinguishable Photon Pairs

We present a theoretical investigation of a whispering gallery mode (WGM) resonator coupled to a Mach-Zehnder interferometer (MZI) and show a bimodal coincidence transmission spectrum when the input state is an indistinguishable photon pair. This is due to the doubled WGM phase shift experienced by the path-entangled state in the interferometer. Further, we model the noise in a WGM resonance shift measurement comparing photon pairs with a coherent state. At least a four-fold improvement in the signal-to-noise ratio (SNR) is possible, with clear implications for quantum-enhanced WGM sensing.

quant-ph

Time-dependent Mandel Q parameter analysis for a hexagonal boron nitride single photon source

The time-dependent Mandel Q parameter, Q(T), provides a measure of photon number variance for a light source as a function of integration time. Here, we use Q(T) to characterise single photon emission from a quantum emitter in hexagonal boron nitride (hBN). Under pulsed excitation a negative Q parameter was measured, indicating photon antibunching at an integration time of 100 ns. For larger integration times Q is positive and the photon statistics become super-Poissonian, and we show by comparison with a Monte Carlo simulation for a three-level emitter that this is consistent with the effect of a metastable shelving state. Looking towards technological applications for hBN single photon sources, we propose that Q(T) provides valuable information on the intensity stability of single photon emission. This is useful in addition to the commonly used $g^{(2)}(τ)$ function for the complete characterisation of a hBN emitter.

quant-ph

Anomalous DNA hybridisation kinetics on gold nanorods revealed via a dual single-molecule imaging and optoplasmonic sensing platform

Observing the hybridisation kinetics of DNA probes immobilised on plasmonic nanoparticles is key in plamon enhanced fluorescence detection from weak emitting species, and refractive index based single-molecule detection on optoplasmonic sensors. The role of the local field in providing plasmonic signal enhancements for single-molecule detection has been studied in great detail. Nevertheless, few studies have compared the experimental results in both techniques for single-molecule studies. Here we developed the first optical setup that integrates optoplasmonic and DNA-PAINT based detection of oligonucleotides to compare these sub-platforms and provide complementary insights into single-molecule processes. We record the fluorescence and optoplasmonic sensor signals for individual, transient hybridisation events. The hybridisation events are observed in the same sample cell and over a prolonged time (i.e. towards high binding site occupancies). A decrease in the association rate over the measurement duration is reported. Our dual optoplasmonic sensing and imaging platform offers insight into the observed phenomenon, revealing that irreversible hybridisation events accumulate over detected step signals in optoplasmonic sensing. Our results point to novel physicochemical mechanisms that result in the stabilisation of DNA hybridisation on optically-excited plasmonic nanoparticles.

physics.optics

Comparing transient oligonucleotide hybridization kinetics using DNA-PAINT and optoplasmonic single-molecule sensing on gold nanorods

We report a comparison of two photonic techniques for single-molecule sensing: fluorescence nanoscopy and optoplasmonic sensing. As the test system, oligonucleotides with and without fluorescent labels are transiently hybridized to complementary docking strands attached to gold nanorods. Comparing the measured single-molecule kinetics helps to examine the influence of fluorescent labels as well as factors arising from different sensing geometries. Our results demonstrate that DNA dissociation is not significantly altered by the fluorescent label, while DNA association is affected by geometric factors in the two techniques. These findings open the door to exploiting plasmonic sensing and fluorescence nanoscopy in a complementary fashion, which will aid in building more powerful sensors and uncovering the intricate effects that influence the behavior of single molecules.

physics.optics

Label-free optical detection of single enzyme-reactant reactions and associated conformational changes

Monitoring the kinetics and conformational dynamics of single enzymes is crucial in order to better understand their biological functions as these motions and structural dynamics are usually unsynchronized among the molecules. Detecting the enzyme-reactant interactions and associated conformational changes of the enzyme on a single molecule basis, however, remain as a challenge with established optical techniques due to the commonly required labeling of the reactants or the enzyme itself. The labeling process is usually non-trivial and the labels themselves might skew the physical properties of the enzyme. Here we demonstrate an optical, label-free method capable of observing enzymatic interactions and the associated conformational changes on the single molecule level. We monitor polymerase/DNA interactions via the strong near-field enhancement provided by plasmonic nanorods resonantly coupled to whispering gallery modes in microcavities. Specifically, we employ two different recognition schemes: one in which the kinetics of polymerase/DNA interactions are probed in the vicinity of DNA-functionalized nanorods, and the other in which these interactions are probed via the magnitude of conformational changes in the polymerase molecules immobilized on nanorods. In both approaches we find that low and high polymerase activities can be clearly discerned via their characteristic signal amplitude and signal length distributions. Furthermore, the thermodynamic study of the monitored interactions suggests the occurrence of DNA polymerization. This work constitutes a proof-of-concept study of enzymatic activities via plasmonically enhanced microcavities and establishes an alternative and label-free method capable of investigating structural changes in single molecules.

physics.bio-ph

Cavity ring-up spectroscopy for ultrafast sensing with optical microresonators

Spectroscopy of whispering-gallery mode (WGM) microresonators has become a powerful scientific tool, enabling detection of single viruses, nanoparticles, and even single molecules. Yet the demonstrated timescale of these schemes has been limited so far to milliseconds or more. Here we introduce a novel scheme that is orders of magnitude faster, capable of capturing complete spectral snapshots of WGM resonances at nanosecond timescales: cavity ring-up spectroscopy (CRUS). Based on sharply-rising detuned probe pulses, CRUS combines the sensitivity of heterodyne measurements with the highest possible, transform-limited acquisition rate. As a demonstration we capture spectra of microtoroid resonators at time intervals as short as 16 ns, directly monitoring sub-microsecond dynamics of their optomechanical vibrations, thermorefractive response and Kerr nonlinearity. CRUS holds promise for the study of fast biological processes such as enzyme kinetics, protein folding and light harvesting, with applications in other fields such as cavity QED and pulsed optomechanics.

physics.optics

Level repulsion in hybrid photonic-plasmonic microresonators for enhanced biodetection

We theoretically analyse photonic-plasmonic coupling between a high Q whispering gallery mode (WGM) resonator and a core-shell nanoparticle. Blue and red shifts of WGM resonances are shown to arise from crossing of the photonic and plasmonic modes. Level repulsion in the hybrid system is further seen to enable sensitivity enhancements in WGM sensors: maximal when the two resonators are detuned by half the plasmon linewidth. Approximate bounds are given to quantify possible enhancements. Criteria for reactive vs. resistive coupling are also established.

physics.optics

Ultrasensitive Detection of a Protein by Optical Trapping in a Photonic-Plasmonic Microcavity

Microcavity and whispering gallery mode (WGM) biosensors derive their sensitivity from monitoring frequency shifts induced by protein binding at sites of highly confined field intensities, where field strengths can be further amplified by excitation of plasmon resonances in nanoparticle layers. Here, we propose a mechanism based on optical trapping of a protein at the site of plasmonic field enhancements for achieving ultra sensitive detection in only microliter-scale sample volumes, and in real-time. We demonstrate femto-Molar sensitivity corresponding to a few 1000s of macromolecules. Simulations based on Mie theory agree well with the optical trapping concept at plasmonic 'hotspots' locations.

physics.optics

Plasmonic Nanoparticle-based Protein Detection by Optical Shift of a Resonant Microcavity

We demonstrated a biosensing approach which, for the first time, combines the high-sensitivity of whispering gallery modes (WGM) with a metallic nanoparticle based assay. We provided a computational model based on generalized Mie theory to explain the higher sensitivity of protein detection through Plasmonic enhancement. We quantitatively analyzed the binding of a model protein (i.e., BSA) to gold nanoparticles from high-Q WGM resonance frequency shifts, and fit the results to an adsorption isotherm, which agrees with the theoretical predictions of a two-component adsorption model.

physics.optics

Lasing in localized modes of a slow light photonic crystal waveguide

We demonstrate lasing in GaAs photonic crystal waveguides with InAs quantum dots as gain medium. Structural disorder is present due to fabrication imperfection and causes multiple scat- tering of light and localization of light. Lasing modes with varying spatial extend are observed at random locations along the guide. Lasing frequencies are determined by the local structure and occur within a narrow frequency band which coincides with the slow light regime of the waveguide mode. The three-dimensional numerical simulation reveals that the main loss channel for lasing modes located away from the waveguide end is out-of-plane scattering by structural disorder.

physics.optics

All-Optical Arithmetic and Combinatorial Logic Circuits with High-Q Bacteriorhodopsin Coated Microcavities

We present designs of all-optical computing circuits, namely, half-full adder/subtractor, de-multiplexer, multiplexer, and an arithmetic unit, based on bacteriorhodopsin (BR) protein coated microcavity switch in a tree architecture. The basic all-optical switch consists of an input infrared (IR) laser beam at 1310 nm in a single mode fiber (SMF-28) switched by a control pulsed laser beam at 532 nm, which triggers the change in the resonance condition on a silica bead coated with BR between two tapered fibers. We show that fast switching of 50 us can be achieved by injecting a blue laser beam at 410 nm that helps in truncating the BR photocycle at the M intermediate state. Realization of all-optical switch with BR coated microcavity switch has been done experimentally. Based on this basic switch configuration, designs of all-optical higher computing circuits have been presented. The design requires 2n-1 switches to realize n bit computation. The proposed designs require less number of switches than terahertz optical asymmetric demultiplexer based interferometer designs. The combined advantages of high Q factor, tunability, compactness and low power control signals, with the flexibility of cascading switches to form circuits, makes the designs promising for practical applications. The design combines the exceptional sensitivities of BR and microcavities for realizing low power circuits and networks. The designs are general and can be implemented (i) in both fiber-optic and integrated optic formats, (ii) with any other coated photosensitive material, or (iii) an externally controlled microresonator switch.

physics.optics

Experimental observation of strong photon localization in disordered photonic crystal waveguides

We demonstrate experimentally that structural perturbations imposed on highly-dispersive photonic crystal-based waveguides give rise to spectral features that bear signatures of Anderson localization. Sharp resonances with the effective Qs of over 30,000 are found in scattering spectra of disordered waveguides. The resonances are observed in a ~20-nm bandwidth centered at the cutoff of slowly-guided Bloch-modes. Their origin can be explained with interference of coherently scattered electromagnetic waves which results in the formation of a narrow impurity (or localization) band populated with spectrally distinct quasistates. Standard photon localization criteria are fulfilled in the localization band.

physics.optics